催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2010年
3期
343-347
,共5页
张轲%周广栋%李菁%程铁欣
張軻%週廣棟%李菁%程鐵訢
장가%주엄동%리정%정철흔
甲烷%二氧化碳%重整%积炭%六铝酸盐%镧%镍%铝%复合氧化物
甲烷%二氧化碳%重整%積炭%六鋁痠鹽%鑭%鎳%鋁%複閤氧化物
갑완%이양화탄%중정%적탄%륙려산염%란%얼%려%복합양화물
methane%carbon dioxide%reforming%carbon deposition%hexaaluminate%lanthanum%nickel%aluminum%composite oxide
利用X射线粉末衍射、氢程序升温还原、X射线光电子能谱和透射电镜技术研究了在低Ni含量和低比表面积六铝酸盐催化剂LaNiAl_(11)O_(19-δ)上CH_4-CO_2重整反应的积炭行为,考察了该催化剂表面积炭的形貌、来源、积炭物种及其反应性能.结果表明,LaNiAl_(11)O_(19-δ)催化剂表面积炭主要由甲烷裂解产生,并以Ni的碳化物形式存在于活性中心Ni的周围.根据积炭物种活化程度的难易可分为C_α,C_β和C_γ三种类型,其中C_α为容易被CO_2消除的化合碳,而C_β和C_γ则是不易被CO_2消除的石墨碳.透射电镜结果表明,C_α以碳纳米管形式分布于催化剂颗粒周围,但金属Ni活性中心仍能暴露于气相中,因而不影响催化剂的活性.
利用X射線粉末衍射、氫程序升溫還原、X射線光電子能譜和透射電鏡技術研究瞭在低Ni含量和低比錶麵積六鋁痠鹽催化劑LaNiAl_(11)O_(19-δ)上CH_4-CO_2重整反應的積炭行為,攷察瞭該催化劑錶麵積炭的形貌、來源、積炭物種及其反應性能.結果錶明,LaNiAl_(11)O_(19-δ)催化劑錶麵積炭主要由甲烷裂解產生,併以Ni的碳化物形式存在于活性中心Ni的週圍.根據積炭物種活化程度的難易可分為C_α,C_β和C_γ三種類型,其中C_α為容易被CO_2消除的化閤碳,而C_β和C_γ則是不易被CO_2消除的石墨碳.透射電鏡結果錶明,C_α以碳納米管形式分佈于催化劑顆粒週圍,但金屬Ni活性中心仍能暴露于氣相中,因而不影響催化劑的活性.
이용X사선분말연사、경정서승온환원、X사선광전자능보화투사전경기술연구료재저Ni함량화저비표면적륙려산염최화제LaNiAl_(11)O_(19-δ)상CH_4-CO_2중정반응적적탄행위,고찰료해최화제표면적탄적형모、래원、적탄물충급기반응성능.결과표명,LaNiAl_(11)O_(19-δ)최화제표면적탄주요유갑완렬해산생,병이Ni적탄화물형식존재우활성중심Ni적주위.근거적탄물충활화정도적난역가분위C_α,C_β화C_γ삼충류형,기중C_α위용역피CO_2소제적화합탄,이C_β화C_γ칙시불역피CO_2소제적석묵탄.투사전경결과표명,C_α이탄납미관형식분포우최화제과립주위,단금속Ni활성중심잉능폭로우기상중,인이불영향최화제적활성.
Carbonaceous deposits formed during the reaction of CO_2 reforming of methane over hexaaluminate LaNiAl_(11)O_(19-δ) catalyst andtheir reactivity were studied by X-ray diffraction, He-temperature-programmed reduction, X-ray photoelectron spectroscopy, and transmission electron microscopy. The deposited carbon was mainly originated from CH_4 decomposition, and it could be classified as three kinds of surface carbon species, I.e. C_α, C_β, and C_γ species on LaNiAl_(11)O_(19-δ).The carbide carbon, C_α, was very active and could be eliminated by CO_2 easily. However, both C_βand C_γ were the graphitic carbon and were difficult to be eliminated by CO_2. It was suggested that C_α was a kind of nanotube-like carbon, which did not affect the catalytic activity of hexaaluminate LaNiAl_(11)O_(19-δ)catalyst.